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Self-electrochemiluminescence of poly[9,9-bis(3‘-(N,N- dimethyl amino)propyl)-2,7-fluorene]-alt- 2,7-(9,9- dioctylfluorene)] and resonance energy transfer to aluminum tris(8-quinolinolate)
摘要： In this paper, the electrochemiluminescence (ECL) behavior of a hole-transport polymer, poly [9,9-bis(3'-(N,N-dimethylamino) propyl)-2,7-fluorene]-alt-2,7-(9,9-dioctylfluorene)] (PFN) was examined with the purpose of finding a novel organic ECL emitter. It was found that the PFN exhibits self-electrochemiluminescence (self-ECL) without any exogenous co-reactants. Quite different from the traditional ECL, the addition of tripropyl amine (TPA) quenched the self-ECL of PFN. PFN ECL intensity reaches a peak during electrochemical oxidation process due to the superposition of self-enhanced ECL, and aggregation quenching of excited state by PFN excimer formation. Aluminum tris(8-quinolinolate) (AlQ3) doped with PFN recovers luminescence intensity with restraining quenching effect via ECL resonance energy transfer from PFN to AlQ3, giving rise to a stable luminescence signal, and hence sensory detection of nitroaromatics. The limits of detections for nitroaromatics can reach down to a level of 10^-22 M. This work sets the stage for a novel organic polymer-based ECL emitter without using any toxic exogenous co-reactant, and presents a practical avenue for a prototype of realising sensory detection through signal stabilization via energy resonance energy transfer (ERET).
关键词： poly[9,9-bis(3'-(N,N-dimethylamino)propyl)-2,7-fluorene]-alt-2,7-(9,9-dioctylfluorene),Sensor,Resonance energy transfer,Self-electrochemiluminescence
更新于2025-09-23 15:23:52
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Influence of the intramolecular donor-acceptor distance on the performance of double-cable polymers
摘要： A series of double-cable polymers PFT-C4-PDI, PFT-C6-PDI and PFT-C8-PDI, composed of the poly(fluorene-alt-thiophene) (PFT) backbone, the perylene diimide (PDI) pendants and the length-various (four-, six- and eight-carbon) covalent alkoxy linkers, were presented. The backbone polymer chain created the hole-transporting channel and the inner-chain aggregation of PDI units created the electron-transporting channel, but the aggregation became weaker along with the longer linker, as proven by the UV-Vis absorption and fluorescence quenching. The polymers were non-conducting, but functioned as efficient compatibilizers. The doping of the polymers induced the formation of the bi-continuous networks inside P3HT:PCBM blends, facilitated photo-generated exciton dissociation and charge transporting. PFT-C4-PDI more efficiently increased the absorption coefficient and the charge-carrier mobility of the P3HT:PCBM film. The power conversation efficiency (PCE) of the P3HT:PCBM bulk-heterojunction solar cells with 3 wt% PFT-C4-PDI, PFT-C6-PDI and PFT-C8-PDI doping were improved by 16.9%, 9.2% and 8.0%, respectively, relative to the non-doped reference device.
关键词： Structure-property relationships,Energy transfer,Double-cable polymer,Polymer solar cells,Bi-continuous networks
更新于2025-09-23 15:23:52
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A new solar hybrid clean fuel-fired distributed energy system with solar thermochemical conversion
摘要： This paper proposes a new solar hybrid clean fuel-fired distributed energy system to increase the system thermodynamic efficiency and save fossil fuel, in which solar energy is upgraded into high-level chemical energy of syngas (H2 and CO) by integrating the solar-driven methanol decomposition based thermochemical conversion. Solar energy, in the form of chemical energy of the generated syngas, is steadily stored and utilized to drive the distributed energy system to generate power, heat and cooling. The double-axis tracking parabolic trough solar collector is deployed to the proposed system to reduce the cosine loss of solar energy. The incorporation of the solar thermochemistry and double-axis solar concentrator technologies leads to a significant improvement in the solar energy utilization efficiency and the off-design performances under varying solar irradiations. With the integration of solar energy utilization and tri-generation, the proposed system achieves a high net solar-to-electric efficiency, 24.66%, and results in high primary energy ratio, 83.86%, exergy efficiency, 38.81%, and carbon emission saving rate, 51.43%. The proposed system is deployed to an office building to study the operation strategies and annual thermo-economy performances, and competitive off-design performances and economy performances are achieved. The research findings open up a new avenue towards the efficient utilization modes of clean fuel and solar energy.
关键词： Distributed energy system,Solar fuel,Solar thermochemistry,Methanol decomposition,Tracking strategy
更新于2025-09-23 15:23:52
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Edge/Defect-rich, Metallic, and Oxygen-heteroatom-doped WS2 Superstructure with Superior Electrocatalytic Performance for Green Solar Energy Conversion
摘要： Two-dimensional tungsten sulfide is widely applied in electrocatalysis field. However, WS2 possesses catalytic active sites located at the layer edge and an inert surface for catalysis. Therefore, increasing the exposure of active sites at the edge and effectively activating the inert sites on the surface is important challenges. Here, we synthesize edge/defect-rich and oxygen-heteroatom-doped WS2 (ED-O-WS2) superstructure. The power-conversion efficiency (PCE) of dye-sensitized solar cells (DSCs) based on ED-O-WS2 counter electrode reach 10.36% (under 1 Sun, AM 1.5, 100 mW cm?2) and 11.19% (under 40 mW cm?2). These values are, to our knowledge, the highest reported efficiency for DSCs based on Pt-free counter electrodes in I3-/I- electrolytes. Analysis of micro-nano structure and electrocatalytic mechanism indicate that ED-O-WS2 exhibit metallic properties in the electrolyte, and that rich edge/defect and oxygen doping in ED-O-WS2 play an important role in improving the catalytic activity of WS2. Moreover, ED-O-WS2 displays better catalytic reversibility for I3-/I- electrolytes than that of noble metal Pt.
关键词： WS2,green solar energy conversion,dye-sensitized solar cells,counter electrode
更新于2025-09-23 15:23:52
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Redox-state dependent blinking of single photosystem I trimers at around liquid-nitrogen temperature
摘要： Efficient light harvesting in a photosynthetic antenna system is disturbed by a ragged and fluctuating energy landscape of the antenna pigments in response to the conformation dynamics of the protein. This situation is especially pronounced in Photosystem I (PSI) containing red shifted chlorophylls (red Chls) with the excitation energy much lower than the primary donor. The present study was conducted to clarify light-harvesting dynamics of PSI isolated from Synechocystis sp. PCC6803 by using single-molecule spectroscopy at liquid?nitrogen temperatures. Fluorescence emission at around 720 nm from the red Chls in single PSI trimers was monitored at 80–100 K. Intermittent variations in the emission intensities, so-called blinking, were frequently observed. Its time scale lay in several tens of seconds. The blinking amplitude depended on the redox state of the phylloquinone (A1). Electrochromic shifts of Chls induced by the negative charge on A1 were calculated based on the X-ray crystallographic structure. A Chl molecule, Chl-A839 (numbering according to PDB 5OY0), bound near A1 was found to have a large electrochromic shift. This Chl has strong exciton coupling with neighboring Chl (A838) whose site energy was predicted to be determined by interaction with an arginine residue (ArgF84) [Adolphs et al., 2010]. A possible scenario of the blinking was proposed. Conformational fluctuations of ArgF84 seesaw the excitation-energy of Chl-A838, which perturbs the branching ratio of excitation-energy between the red Chl and the cationic form of P700 as a quencher. The electrochromic shift of Chl-A839 enhances the effect of the conformation dynamics of ArgF84.
关键词： Cryogenic microscope,Phylloquinone,Fluorescence blinking,Site energy,Single-molecule spectroscopy,Electrochromic shift
更新于2025-09-23 15:23:52
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Phononic Casimir corrections for Graphene resonator
摘要： By calculating a Casimir energy for the acoustic phonons of Graphene, we find some temperature-dependent corrections for the pretension of a Graphene sheet suspended on a trench. We obtain values of the order of few mN/m for these corrections in fully as well as doubly clamped Graphene on a narrow trench with one nanometer width, at room temperature. These values are considerable compared to the experimental values, and can increase the fundamental resonance frequency of the Graphene. The values of these corrections increase by increasing the temperature, and so they can be utilized for tuning the Graphene pretension.
关键词： Resonance frequency,Graphene sheet,Casimir energy,Acoustic phonons,Pretension,Nanoelectromechanical systems
更新于2025-09-23 15:23:52
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Enhancing pyroelectric properties in (Pb1-1.5La )(Zr0.86Ti0.14)O3 ceramics through composition modulated phase transition
摘要： Currently, there is an urgent need of extraordinary comprehensive pyroelectric materials for the wide application in detectors and energy harvesters. In this study, the (Pb1-1.5xLax)(Zr0.86Ti0.14)O3 (abbreviated as PLZT, x = 0.02, 0.03, 0.04 and 0.05) ceramics located in ferroelectric-antiferroelectric (FE-AFE) phase boundary were designed and synthesized by using conventional solid-state reaction method. The microstructures, phase structures, dielectric, ferroelectric, thermal depolarization and pyroelectric properties of the PLZT ceramics with different La content were investigated thoroughly. The XRD results show that the PLZT ceramics change from FE phase to AFE phase with increasing La content. The significant improvement of pyroelectric coefficient and figures of merit (FOMs) are achieved in the PLZT ceramics with the increase in La content because of the increased metastable ferroelectric phase under the application of electric field. The (Pb0.955La0.03)(Zr0.86Ti0.14)O3 (x = 0.03) ceramic exhibits not only high of and high depolarization temperature (Td) of 179 ℃ but also excellent FOMs with ???? = , ???? = , and ???? = 3 47 5 ???? ? . In addition, the highest of is achieved in (Pb0.94La0.04)(Zr0.86Ti0.14)O3 (x = 0.04) ceramic. These results demonstrate that the PLZT ceramics of x = 0.03 and 0.04 are promising candidates for pyroelectric applications.
关键词： ferroelectric/antiferroelectric material,energy harvesting,(Pb,La)(Zr,Ti)O3 ceramics,pyroelectric properties
更新于2025-09-23 15:23:52
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Diffusion of Ar atoms implanted in a TiO2 matrix studied with Temperature Programmed Out-Diffusion?
摘要： The diffusion of noble gas argon in the near-surface region of rutile TiO2 has been explored with the Temperature Programmed Out-Diffusion (TPOD) method. The Ar atoms were deposited in a several-nanometer-deep layer of the single-crystal TiO2(110) surface by bombardment with 1–5 keV energy Ar ions. Subsequently, in the TPOD experiments this sample was heated at a linear rate and the out-diffusion of argon was monitored with a mass-spectrometer. Surface conditions were probed with Auger Electron Spectroscopy (AES) and Low-Energy Electron Diffraction (LEED). The experimental results were analyzed with the aid of numerical simulations. The measurements showed a dependence of the Ar diffusion rates on the concentration of buried argon and composition of the surface layer. The kinetic parameters of Ar diffusion in pristine rutile TiO2 were estimated as Ea = 104 kJ/mol and D0 = 6 ? 10?9 m2/s. A distinctive diffusion regime, related to the rock salt TiO phase formation, were identified.
关键词： Sputtering,TiO2,Low-energy ion implantation,Solid diffusion,Ar
更新于2025-09-23 15:23:52
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Concentration effects on the thermally-activated transport of polarons in conducting polymers
摘要： The impact of the polaron concentration on the temperature-mediated charge transport in one-dimensional organic materials is studied. Within the scope of a tight-binding description, our findings reveal that high-temperature diffusivity tends to increase as polaron concentration increases. Moreover, the activation energy for the polaron transport also increases with polaron concentration. Importantly, the polaron diffusivity follows an Arrhenius-like behavior with low activation energy.
关键词： Activation energy,Organic materials,Polaron concentration,Diffusivity
更新于2025-09-23 15:23:52
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Raman/XRF/EDX microanalysis of 2nd-century stuccoes from Domus Valeriorum in Rome
摘要： 2nd-century stucco fragments from the roman Domus Valeriorum were analyzed by Raman spectroscopy (Raman), imaging X-ray fluorescence (XRF) and energy dispersive X-ray microanalysis (EDX) in order to identify the pigments and materials thereon. Cinnabar, malachite, hematite, goethite and Egyptian blue were detected by the synergistic use of these techniques whereas calcite, with some traces of gypsum, was detected as materials for the bas-relief figures and the pictorial background. This non-destructive characterization is the first carried out on the Domus Valeriorum finds. The multi-analytical approach highlighted the complementarity and versatility of these techniques, suitable for both laboratory and in-situ analysis, on macroscopic or microscopic fragments without preliminary manipulation.
关键词： Energy dispersive X-ray fluorescence,X-ray fluorescence imaging,Domus Valeriorum,Pigments,Raman spectroscopy
更新于2025-09-23 15:23:52